TY - JOUR
T1 - From Fundamental Theories to Quantum Coherences in Electron Transfer
AU - Rafiq, Shahnawaz
AU - Scholes, Gregory D.
N1 - Publisher Copyright:
Copyright © 2018 American Chemical Society.
PY - 2019/1/16
Y1 - 2019/1/16
N2 - Photoinduced electron transfer (ET) is a cornerstone of energy transduction from light to chemistry. The past decade has seen tremendous advances in the possible role of quantum coherent effects in the light-initiated energy and ET processes in chemical, biological, and materials systems. The prevalence of such coherence effects holds a promise to increase the efficiency and robustness of transport even in the face of energetic or structural disorder. A primary motive of this Perspective is to work out how to think about "coherence" in ET reactions. We will discuss how the interplay of basic parameters governing ET reactions - like electronic coupling, interactions with the environment, and intramolecular high-frequency quantum vibrations - impact coherences. This includes revisiting the insights from the seminal work on the theory of ET and time-resolved measurements on coherent dynamics to explore the role of coherences in ET reactions. We conclude by suggesting that in addition to optical spectroscopies, validating the functional role of coherences would require simultaneous mapping of correlated electron motion and atomically resolved nuclear structure.
AB - Photoinduced electron transfer (ET) is a cornerstone of energy transduction from light to chemistry. The past decade has seen tremendous advances in the possible role of quantum coherent effects in the light-initiated energy and ET processes in chemical, biological, and materials systems. The prevalence of such coherence effects holds a promise to increase the efficiency and robustness of transport even in the face of energetic or structural disorder. A primary motive of this Perspective is to work out how to think about "coherence" in ET reactions. We will discuss how the interplay of basic parameters governing ET reactions - like electronic coupling, interactions with the environment, and intramolecular high-frequency quantum vibrations - impact coherences. This includes revisiting the insights from the seminal work on the theory of ET and time-resolved measurements on coherent dynamics to explore the role of coherences in ET reactions. We conclude by suggesting that in addition to optical spectroscopies, validating the functional role of coherences would require simultaneous mapping of correlated electron motion and atomically resolved nuclear structure.
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U2 - 10.1021/jacs.8b09059
DO - 10.1021/jacs.8b09059
M3 - Review article
C2 - 30412671
AN - SCOPUS:85057814730
SN - 0002-7863
VL - 141
SP - 708
EP - 722
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 2
ER -